skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: All-perovskite tandem solar cells with improved grain surface passivation

Journal Article · · Nature (London)

All-perovskite tandem solar cells hold the promise of surpassing the efficiency limits of single-junction solar cells; however, until now, the best-performing all-perovskite tandem solar cells have exhibited lower certified efficiency than have single-junction perovskite solar cells. A thick mixed Pb–Sn narrow-bandgap subcell is needed to achieve high photocurrent density in tandem solar cells, yet this is challenging owing to the short carrier diffusion length within Pb–Sn perovskites. Here we develop ammonium-cation-passivated Pb–Sn perovskites with long diffusion lengths, enabling subcells that have an absorber thickness of approximately 1.2 μm. Molecular dynamics simulations indicate that widely used phenethylammonium cations are only partially adsorbed on the surface defective sites at perovskite crystallization temperatures. The passivator adsorption is predicted to be enhanced using 4-trifluoromethyl-phenylammonium (CF3-PA), which exhibits a stronger perovskite surface-passivator interaction than does phenethylammonium. By adding a small amount of CF3-PA into the precursor solution, we increase the carrier diffusion length within Pb–Sn perovskites twofold, to over 5 μm, and increase the efficiency of Pb–Sn perovskite solar cells to over 22%. Here, we report a certified efficiency of 26.4% in all-perovskite tandem solar cells, which exceeds that of the best-performing single-junction perovskite solar cells. Encapsulated tandem devices retain more than 90% of their initial performance after 600 h of operation at the maximum power point under 1 Sun illumination in ambient conditions.

Research Organization:
Univ. of Kentucky, Lexington, KY (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Key Research and Development Program of China; National Natural Science Foundation of China (NSFC); Natural Science Foundation of Jiangsu Province; US Department of the Navy, Office of Naval Research
Grant/Contract Number:
SC0018208; 2018YFB1500102; 61974063; 61921005; BK20202008; BK20190315; N00014-20-1-2572
OSTI ID:
2204711
Journal Information:
Nature (London), Vol. 603, Issue 7899; ISSN 0028-0836
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English

References (48)

Perovskite solar cells: On top of commercial photovoltaics journal January 2017
Prospects for metal halide perovskite-based tandem solar cells journal May 2021
Monolithic Perovskite Tandem Solar Cells: A Review of the Present Status and Advanced Characterization Methods Toward 30% Efficiency journal May 2020
Monolithic all-perovskite tandem solar cells with 24.8% efficiency exploiting comproportionation to suppress Sn(ii) oxidation in precursor ink journal September 2019
Perovskite solar cells with atomically coherent interlayers on SnO2 electrodes journal October 2021
Enhancing electron diffusion length in narrow-bandgap perovskites for efficient monolithic perovskite tandem solar cells journal October 2019
Perovskite-perovskite tandem photovoltaics with optimized band gaps journal October 2016
Cost Analysis of Perovskite Tandem Photovoltaics journal August 2018
Solar cell efficiency tables (Version 58)
  • Green, Martin A.; Dunlop, Ewan D.; Hohl‐Ebinger, Jochen
  • Progress in Photovoltaics: Research and Applications, Vol. 29, Issue 7 https://doi.org/10.1002/pip.3444
journal June 2021
All-perovskite tandem solar cells with 24.2% certified efficiency and area over 1 cm2 using surface-anchoring zwitterionic antioxidant journal October 2020
Carrier lifetimes of >1 μs in Sn-Pb perovskites enable efficient all-perovskite tandem solar cells journal April 2019
Simplified interconnection structure based on C60/SnO2-x for all-perovskite tandem solar cells journal July 2020
Low-bandgap mixed tin–lead iodide perovskites with reduced methylammonium for simultaneous enhancement of solar cell efficiency and stability journal October 2020
Modulated Crystallization and Reduced V OC Deficit of Mixed Lead–Tin Perovskite Solar Cells with Antioxidant Caffeic Acid journal July 2021
Tin‐Lead Perovskite Fabricated via Ethylenediamine Interlayer Guides to the Solar Cell Efficiency of 21.74% journal May 2021
What Makes a Good Solar Cell? journal March 2018
Classification of solar cells according to mechanisms of charge separation and charge collection journal January 2015
Defect and Contact Passivation for Perovskite Solar Cells journal April 2019
Response to Comment on “Resolving spatial and energetic distributions of trap states in metal halide perovskite solar cells” journal February 2021
Top and bottom surfaces limit carrier lifetime in lead iodide perovskite films journal January 2017
Instability of Tin Iodide Perovskites: Bulk p-Doping versus Surface Tin Oxidation journal July 2020
Optoelectronic Properties of Tin–Lead Halide Perovskites journal June 2021
Lewis-Adduct Mediated Grain-Boundary Functionalization for Efficient Ideal-Bandgap Perovskite Solar Cells with Superior Stability journal August 2018
Minimizing non-radiative recombination losses in perovskite solar cells journal November 2019
Recent Progresses on Defect Passivation toward Efficient Perovskite Solar Cells journal April 2020
Materials and Methods for Interface Engineering toward Stable and Efficient Perovskite Solar Cells journal July 2020
Vertically Aligned 2D/3D Pb–Sn Perovskites with Enhanced Charge Extraction and Suppressed Phase Segregation for Efficient Printable Solar Cells journal April 2020
Surface Ligands for Methylammonium Lead Iodide Films: Surface Coverage, Energetics, and Photovoltaic Performance journal February 2020
Constructive molecular configurations for surface-defect passivation of perovskite photovoltaics journal December 2019
Combining Efficiency and Stability in Mixed Tin–Lead Perovskite Solar Cells by Capping Grains with an Ultrathin 2D Layer journal March 2020
Imperfections and their passivation in halide perovskite solar cells journal January 2019
Surface passivation of perovskite film for efficient solar cells journal April 2019
Supramolecular Halogen Bond Passivation of Organic–Inorganic Halide Perovskite Solar Cells journal May 2014
Self-Regulation Mechanism for Charged Point Defects in Hybrid Halide Perovskites journal December 2014
High Charge Carrier Mobilities and Lifetimes in Organolead Trihalide Perovskites journal December 2013
Minority and Majority Charge Carrier Mobility in Cu2ZnSnSe4 revealed by Terahertz Spectroscopy journal September 2018
Monolithic perovskite/silicon tandem solar cell with >29% efficiency by enhanced hole extraction journal December 2020
Enabling Flexible All-Perovskite Tandem Solar Cells journal September 2019
Thermally Stable All‐Perovskite Tandem Solar Cells Fully Using Metal Oxide Charge Transport Layers and Tunnel Junction journal October 2021
CP2K: An electronic structure and molecular dynamics software package - Quickstep: Efficient and accurate electronic structure calculations journal May 2020
A unified formulation of the constant temperature molecular dynamics methods journal July 1984
Gaussian basis sets for accurate calculations on molecular systems in gas and condensed phases journal September 2007
Separable dual-space Gaussian pseudopotentials journal July 1996
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set journal October 1996
Generalized Gradient Approximation Made Simple journal October 1996
Multiwfn: A multifunctional wavefunction analyzer journal December 2011
Low-temperature processed inorganic hole transport layer for efficient and stable mixed Pb-Sn low-bandgap perovskite solar cells journal October 2019
GenPro4 Optical Model for Solar Cell Simulation and Its Application to Multijunction Solar Cells journal May 2017